the effect of four methods of surface activation for

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PRIFYSGOL BANGOR / BANGOR UNIVERSITY The effect of four methods of surface activation for improved adhesion of wood polymer composites (WPCs) Dimitriou, Athanasios; Hale, Michael; Spear, Morwenna International Journal of Adhesion and Adhesives DOI: 10.1016/j.ijadhadh.2016.03.003 Published: 01/07/2016 Version created as part of publication process; publisher's layout; not normally made publicly available Cyswllt i'r cyhoeddiad / Link to publication Dyfyniad o'r fersiwn a gyhoeddwyd / Citation for published version (APA): Dimitriou, A., Hale, M., & Spear, M. (2016). The effect of four methods of surface activation for improved adhesion of wood polymer composites (WPCs). International Journal of Adhesion and Adhesives, 68(July), 188-194. https://doi.org/10.1016/j.ijadhadh.2016.03.003 Hawliau Cyffredinol / General rights Copyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights. • Users may download and print one copy of any publication from the public portal for the purpose of private study or research. • You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal ? Take down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. 06. Nov. 2021

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Page 1: The effect of four methods of surface activation for

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The effect of four methods of surface activation for improved adhesion ofwood polymer composites (WPCs)Dimitriou, Athanasios; Hale, Michael; Spear, Morwenna

International Journal of Adhesion and Adhesives

DOI:10.1016/j.ijadhadh.2016.03.003

Published: 01/07/2016

Version created as part of publication process; publisher's layout; not normally made publiclyavailable

Cyswllt i'r cyhoeddiad / Link to publication

Dyfyniad o'r fersiwn a gyhoeddwyd / Citation for published version (APA):Dimitriou, A., Hale, M., & Spear, M. (2016). The effect of four methods of surface activation forimproved adhesion of wood polymer composites (WPCs). International Journal of Adhesion andAdhesives, 68(July), 188-194. https://doi.org/10.1016/j.ijadhadh.2016.03.003

Hawliau Cyffredinol / General rightsCopyright and moral rights for the publications made accessible in the public portal are retained by the authors and/orother copyright owners and it is a condition of accessing publications that users recognise and abide by the legalrequirements associated with these rights.

• Users may download and print one copy of any publication from the public portal for the purpose of privatestudy or research. • You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal ?

Take down policyIf you believe that this document breaches copyright please contact us providing details, and we will remove access tothe work immediately and investigate your claim.

06. Nov. 2021

Page 2: The effect of four methods of surface activation for

Author’s Accepted Manuscript

The effect of four methods of surface activation forimproved adhesion of wood polymer composites(WPCs)

A. Dimitriou, M.D. Hale, M.J. Spear

PII: S0143-7496(16)30049-5DOI: http://dx.doi.org/10.1016/j.ijadhadh.2016.03.003Reference: JAAD1806

To appear in: International Journal of Adhesion and Adhesives

Received date: 29 January 2015Accepted date: 4 February 2016

Cite this article as: A. Dimitriou, M.D. Hale and M.J. Spear, The effect of fourmethods of surface activation for improved adhesion of wood polymercomposites (WPCs), International Journal of Adhesion and Adhesives,http://dx.doi.org/10.1016/j.ijadhadh.2016.03.003

This is a PDF file of an unedited manuscript that has been accepted forpublication. As a service to our customers we are providing this early version ofthe manuscript. The manuscript will undergo copyediting, typesetting, andreview of the resulting galley proof before it is published in its final citable form.Please note that during the production process errors may be discovered whichcould affect the content, and all legal disclaimers that apply to the journal pertain.

www.elsevier.com/locate/ijadhadh

Page 3: The effect of four methods of surface activation for

The effect of four methods of surface activation for improved adhesion of wood polymer

composites (WPCs)

A. Dimitriou, M. D. Hale and M. J. Spear*

College of Natural Sciences, Bangor University, Bangor, LL57 2UW, UK

[email protected]

[email protected]

[email protected]

+44 1248 382029

*corresponding author

Keywords

Wood Plastic Composites, lap shear, surface treatment, adhesion

Page 4: The effect of four methods of surface activation for

Abstract

Wood Polymer Composites (WPCs) have attracted a lot of interest in recent years as materials with a

high renewable content. However the adhesion between WPC components is problematic because

of low surface energy and the hydrophobic nature of the most widely used polymer matrices, i.e.

polyolefins. Thus this paper has looked at four surface activation pretreatment methods to improve

adhesion properties for bonding using epoxy adhesives, namely: hydrogen peroxide solution; hot air;

a gas flame; and halogen heating lamps. The treatments were applied to WPC materials made from

60% wood flour in a polypropylene matrix, and lap joint shear strength was measured.

Shear strength values showed that all treatments except the halogen heating lamps increased the

bond strength and the best results were achieved with hydrogen peroxide treatment at a pH of 7.5

(37% improvement); a two pass hot air treatment at a pass speed of 75 mm s-1 (44% improvement);

and a gas flame treatment at a pass speed of 175 mm s-1(41 % improvement).The bond strength was

increased to values that caused failure within the material, rather than at the interfaces of the bond

line.

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1. Introduction

Wood Polymer Composites (WPCs) are materials which are composed of lignocellulosic fibres and

thermoplastic polymers in varying percentages [1]. Typically, solid profiles are formed by extrusion,

and this material is suitable for mechanical jointing and bonding by traditional wood jointing

techniques, but adhesion between components is currently poor. During recent years there has

been special interest in developing plastics made using lignocellulose fibres as reinforcing fillers [2]

and to reduce raw material costs. Although these improvements are not new developments the

material is essentially renewable [3] and can be made employing recycled polymer and wood

industry waste [4].

The most commonly used polymers for WPC production are the polyolefins – low density

polyethylene (LDPE), high density polyethylene (HDPE), polypropylene (PP), polyvinyl chloride (PVC)

and polystyrene (PS) [1, 2, 5], which are suitable because of their low processing temperature. High

processing temperatures (above 200°C) can cause thermal decomposition of the lignocellulosic

reinforcement [3, 5]. Polyolefin wastes arise as a solid waste stream from cities, e.g. packaging

materials, thus the re-use as matrix polymer for WPCs can provide green benefits [6]. The

mechanical properties of recycled polymer WPCs are similar to those made from virgin polymers and

in some instances, are better [7].

Jointing of WPCs normally uses mechanical fasteners which have been developed for wood, metal

and polymeric materials [8]. On the other hand glued joints in WPCs can show poor adhesion

properties, in the same manner as the native unfilled polyolefins. This is because of the limited

wettability and low surface energy of the polyolefin matrix polymers [9] and this can be problematic

in designing products such as furniture from WPC materials. In order to improve adhesion ability of

polyolefins, surface activation treatments such as oxidative pre-treatments are essential [10, 11], but

there are few studies in this area for WPC materials. The most common pre-treatments already used

in the polymer industry are chemical, flame, corona, plasma and UV irradiation treatments [11, 12].

Other treatments like fluorination, oxy-fluorination and microwave irradiation are also effective for

surface oxidation, which result in the improvement in adhesion [13, 14].

Moghadamzadeh et al. [15] clearly demonstrated that mechanical surface preparation by sanding

altered the WPC surface from a polymer rich to a more wood-rich substrate. Sanding is a routine

surface preparation technique in the wood furniture sector and has been applied to all samples

including the control in this study. Also specifically for WPCs, Oporto and co-workers [10] performed

a series of chemical, mechanical, energetic and physical pre-treatments (chromic acid, surface

sanding, flame treatment, heat treatment, water, and combination of water-flame treatments).

Almost all of the tested methods showed an improvement in the adhesion strength of their 50.4%

pine, 39.6% PP composite. Heat treatment using a hot air gun was the only case where the adhesion

strength was reduced. These improvements were recorded against unsanded control samples.

A greater number of studies have addressed the use of corona and plasma treatments for WPC

materials [10, 12, 15, 16, 17, 18] than have investigated mechanical [10, 15] or flame [15, 19] or

chemical [10, 12, 20] treatments for WPCs. Plasma and flame treatment options are suitable for use

in factory production, however many WPC applications utilise relatively low investment technology,

and a workshop scale of production. Flame and other sources of heat were considered to have

potential for furniture manufacture within this context.

Due to its relatively high cost epoxy resin is a less commonly used adhesive for wood jointing in

furniture industry [21], however it is widely used for polymer composites. Many researchers [10, 15,

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19, 20] have used epoxy resin as the adhesion system for studies on WPC materials. A preliminary

study on WPC materials [22] had compared lap shear strength of epoxy with the more traditional

wood glues: PVA and polyurethane. In these tests epoxy outperformed PVA by 243.6% and PU by

198%, so was selected for use in the surface activation study.

In this study hydrogen peroxide and halogen heating lamps were chosen, alongside hot air and flame

pretreatments. These were examined for surface oxidation and adhesion improvement. All the

selected methods were chosen as safe and easily applicable procedures that could performed in a

small workshop without the need of expensive, sophisticated equipment. The hot air gun, flame and

halogen heating lamps were expected to activate the WPC surface as a result of the thermal

degradation of the polymer. This mechanism is known to involve free radical formation by the action

of heat. This may proceed by initiation and propagation as follows:

Polymer → P• + P•

P• + O2 → POO•

POO• + PH → POOH + P•

Peroxides are well known to form oxidative free radicals and are used for surface bleaching and

surface colour modifications for wood [23] and thus suitable for surface application. Hydrogen

peroxide forms a hydroperoxy radical OOH• which causes the surface oxidation as follows:

H2O2 H• + OOH•

OOH• + R• → ROOH

The OOH• radicals react with the material surface in the presence of an activator and significantly

increases the surface polarity. NaOH is the most commonly used activator for controlling the pH of

the treatment solution [23].

2. Materials and Methods

A WPC containing 60% Norway spruce flour, 35.5% polypropylene, 2% coupling agent, 1.5% UV-

stabilizer and 1% colour pigment sourced from Kompetenzzentrum Holz GmbH Austria. This was

produced under the European research project ERA-NET Cornet/2006/01. The WPC was an extruded

square shaped pipe, allowing samples to be cut from the sides. 30% w/v H2O2 and 1M NaOH were

obtained from Panreac Quimica SAU. A rapid curing two component commercial epoxy resin

adhesive (Saldatutto mix) from Pattex was used for lap joint bonding.

WPC samples were cut with dimensions 40 mm X 20 mm X 5 mm and all samples were sanded with

P220 glass paper to abrade the surface to produce a uniform surface for bonding. The samples were

rinsed with deionised water after sanding to remove any remaining sanding dust on the surface,

similarly, samples were rinsed after every surface activation treatment. Rinsing has been shown to

have no significant effect on retention of surface activation for flame-treated polypropylene [24],

and was required in this study to remove surplus treatment solution from the peroxide treated

samples. They were conditioned at 20°C and 65% RH (relative humidity) to constant weight before

treatment, and again afterwards. After each thermal treatment system (hot air, flame and halogen

lamps), the samples were returned to the conditioning chamber to cool for 15 minutes before the

rinsing step. The samples were then conditioned again to constant weight (2 weeks) before bond

formation.

2.2. Surface pretreatments

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Four pre-treatments were evaluated to determine whether they improved bond strength: a

hydrogen peroxide treatment; a hot air treatment; a flame treatment and a halogen lamp treatment.

Within each treatment, variables were examined to give different treatment intensities, and at each

variable 20 replicates were included, giving a total of 560 samples tested. In addition 20 control

samples were prepared by sanding and conditioning, and used as the untreated control set for each

of the four pretreatment methods.

2.2.1. H2O2 treatments

A 30% H2O2 solution was used for the treatments at a series of pH steps from neutral, +/-2. The pH

of the treatment solution was adjusted to 5, 6, 6.5, 7, 7.5, 8, 8.5 and 9 with NaOH. All treatments

were performed at 20°C. The samples were soaked in the treatment solution for 30 minutes, then

washed with deionised water and reconditioned to constant weight.

2.2.2. Hot air treatment

The samples were placed on a steel plate under the hot air gun. A DEWALT DW 340K 2000 W hot air

gun was fixed to a STAUBLI TX90 robotic arm which was programmed to pass in a straight line

direction over the WPC sample surfaces at a range of velocities (in mm s-1: 18.5, 25, 31, 37.5, 67.5,

75, and 115). Thus more intense heating was achieved at slow pass velocities. A double pass at 75

mm s-1 (2X75 mm s-1) was also included for comparison. The distance between the sample surface

and the hot air gun nozzle was fixed to 25 mm.

2.2.3. Flame treatment

In this treatment a MAPP gas flame torch was used, attached to the same robotic arm as for the hot

air samples, but the vertical distance between the nozzle and sample surfaces was set to 50 mm and

the pass velocities were faster (in mm s -1: 125, 150, 175, 200, 225 and 250).

2.2.4. Halogen heating lamps treatment

For the halogen heating lamp treatment, three 400 W 20 cm long halogen heat lamps were

combined to form a linear array with a spacing distance of 80 mm between them and the array unit

was attached to the robotic arm 20 mm above the WPC sample surfaces. Samples were treated at

slow pass velocities (in mm s-1: 10, 20, 30, 40 and 50).

2.3. Lap joint preparation

The adhesive resin and hardener were mixed at a 1:1 w/w ratio and applied to both sample surfaces

of the lap joint under laboratory conditions at 20°C. Then the joints were gripped with pneumatic

clamps under equal pressure for 15 minutes to ensure sample uniformity within and between

treatment groups. The bonding area was 10 mm X 20 mm (Figure 1a). All samples then conditioned

as above for 48 hours.

Page 8: The effect of four methods of surface activation for

Figure 1. (a) Lap joint assembly (b) adhesive failure during shear test (c) material cohesive failure

during shear test.

2.4. Shear testing of lap joints

For the bonding shear strength evaluation a Zwick/Roell Z020 universal testing machine was used.

The mechanical properties were determined according to EN 205:2003 [25] using a 1.5 mm min-1

cross head speed. The sample length was altered to accommodate the available dimensions of

material (Figure 1a), but a lap joint area of 200 mm2 was achieved as required. Mean lap-joint shear

strength values were calculated using data from only samples where failure occurred in the glue

joint. Analysis of the full sample set, including samples which showed material failure, was also

conducted, and will be discussed where relevant in the text.

2.5. Statistical analysis

SPSS statistics version 17.0 software was used to carry out one way ANOVA treated and untreated

control samples’ shear strength values. The shear strength values were analysed with the treatment

factors and untreated material (control) as the independent variable. Homogeneity variance, F-test

and Tukey post hoc HSD multiple comparison test were performed to investigate the possible

statistically significant differences within treatment factors compared to the control.

2.6. Scanning Electron Microscopy

Additional samples were prepared for each surface pre-treatment technique. Pieces of pre-treated

WPC were cut to 20 x 20 mm for Scanning Electron Microscopy (SEM), mounted on stubs and carbon

coated under vacuum (JEOL JEE-4X vacuum evaporator). A JEOL JMS 840A SEM was used to collect

primary (backscattered) and secondary electron images.

3. Results

The shear strength results (Figure 2) showed adhesion strength improvements for all treatments as

compared to the controls, except the halogen heating lamps, which gave lowered adhesion strength

Page 9: The effect of four methods of surface activation for

at all speeds tested. The optimal treatment for each type of surface activation (hydrogen peroxide,

hot air gun and flame) gave similar mean results (where all of the data is included) within the range

of 801-836 N and gives proportional improvements in the order of 37-44%; all of these were

considerable improvements. In some instances, where high increases in bond shear strength

occurred, appreciable numbers of failures occurred within the material, although this was not

statistically significant when tested by Tukey HSD test.

a: Hydrogen peroxide b: Hot air gun

c: Flame d: Halogen heating lamps

Figure 2: Lap joint shear strength (N) of the four treatments. In each graph the horizontal dotted line

presents the control mean value (555 N) and the solid horizontal lines the standard deviation (SD) of the

control values. Error bars represent the SD (+/- 1). a) Hydrogen peroxide treatment. b) Hot air gun

treatment. The mean value of the hot air gun at the 150 mm s-1

treatment speed refers to the samples

treated twice with the speed of 75 mm s-1

. c) Flame treatment and d) Halogen heating lamp treatment.

3.1. Hydrogen peroxide treatment Lap-joint shear strength results

Hydrogen peroxide treatment significantly improved bond shear strength at some pH values (6, 7.5,

8 and 8.5, according to Tukey HSD test) but not at others, and at pH values of 7 and 9 they were

350

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4 5 6 7 8 9

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Solution pH

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0 10 20 30 40 50

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equal or worse than the controls. (Figure 2a). Those better than the controls, pH 6, 7.5, 8 and 8.5,

had similarly high values of over 700 N (no significant difference, Tukey HSD test); overall the highest

bond strength was seen at pH 7.5.

A large number, 80% of the of the pH 7.5 samples, failed by fracture within the WPC material rather

than at the bond line, leading to their exclusion from the calculated mean value and standard

deviation, according to the chosen EN 205 protocol. In the WPC samples the failure within the

material occurred as a cohesive failure within the material immediately adjacent to the bonded area

as shown in Figure 1c. This is similar to the failure which would be expected in the beech wood

substrate commonly used in this test protocol. The EN 205 test [25] is predominantly used to

evaluate the performance of adhesives, so failure in the material indicates the adhesive to be

stronger than the substrate. Analysis of the shear strength values for the samples which showed

material failure, revealed that failure occurred at a higher stress (809 N) than the samples which

failed in the bond line (760 N) and the high failure rate (80%) within the pH 7.5 H2O2 treated WPC

contrasts with only a 5% failure with control samples. This emphasises the good bonding with

peroxide surface treatment at pH 7.5. Other peroxide treatments which showed modest increases of

the within material failures (25%, 40%) were at the slightly higher pH values of 8 and 8.5 respectively

and indicates little or no deterioration in the strength of the WPC substrate at these pH values as a

result of the treatment.

3.2. Hot air treatment

The hot air treatments at the faster pass velocities of 67-115 mm s-1 and the double pass of 2 x 75

mm s-1 also had a positive effect on the adhesion shear strength (Tukey HSD multiple comparison

test). In general the slower speeds gave less positive results, but only the 25 mm s-1 was significantly

better than the controls (Figure 2.b).

It is interesting to note that the samples treated by two passes of the hot air at treatment pass

speed of 75 mm s-1 (75 x 2, Table 1) showed an improvement over those treated with a single pass at

the same speed. The double pass of 75 mm s-1 also gave the highest bond shear strength amongst all

of the surface treatment investigated in this study, and the use of multiple passes warrants further

investigation.

The double pass and the fast treatment speed of 115 mm s-1 showed higher failure rates within the

WPC (50%) which was, as with peroxide treatment at pH 7.5-8.5, associated with high adhesion

shear strength values, in contrast to lower values at lower treatment speeds (Table 1). Conversely

the samples treated at 18.5 mm s-1 had lower bond strengths than the control samples and higher

material failure, which is an indication of material degradation. In scanning electron microscopy

studies distinct differences were observed in the surface for the heat treated samples (Figure 3b).

These were smoother than the control, possibly indicating spreading of the polymer under the heat,

reducing the prominence of sanding marks seen in the control (Figure 3a).

Table 1: Shear strength (N) of samples surface modified at different pass velocities of hot air and

percentages of samples which failed within the material rather than at the glue-line.

Property Control Treatment velocity (mm s-1

)

18.5 25 31 37.5 67 75 115 75 (X2)

Shear strength (N) (EN205) 555 467 719 596 615 707 666 768 798

Within material failure (%) 5 10 5 30 30 25 25 50 50

Shear strength all samples (N) 566 493 730 673 674 743 686 789 836

Page 11: The effect of four methods of surface activation for

a: b:

Figure 3: Backscattered electron image of a) rough texture in sanded control sample and b) hot air

treated sample (18.5 mm s-1

) where polymer surface (darker areas) appears smoother due to the action of

heat.

3.3. Flame treatment

Of the six different flame treatment pass speeds, from 125 to 250 mm s-1, only two clearly and

significantly (Tukey HSD test) improved the adhesion strength (Figure 2c, 175 mm s-1 and 250 mm s-1)

but all treatments except the slowest velocity (125 mm s-1) had a positive effect. High variation in the

data gave insignificant differences for the other velocities. As well as giving the highest bond

strengths, the samples treated at 175 mm s-1 also had a higher percentage of material failure (65%)

rather than at the bond line. This further indicates that 175 mm s-1 is the optimal treatment velocity

(Table 2). As expected, the samples with decreasing lap shear strengths showed progressively lower

percentage material failures.

Table 2: Shear strength (N) of samples surface modified at different pass velocities of a flame and

percentages of samples which failed within the material rather than at the glue-line.

Control Treatment velocity (mm s-1

)

Property 125 150 175 200 225 250

Shear strength (N) (EN205) 555 472 649 782 621 616 674

Within material failure (%) 5 0 20 65 10 5 25

Shear strength all samples (N) 566 472 666 841 641 631 704

3.4. Halogen heating lamps treatment

All of the halogen heat lamp treated samples had reduced bond strengths and high variability (Figure

2d), with mean values ranging from 451 to 487 N, some 12-19% less than the controls. No material

failure was observed among the treated samples, probably due to the weakness of the bond.

According to the Tukey HSD multiple comparison test, all the samples treated with the halogen

heating lamp were significantly statistically different to the untreated control and there were no

statistically significant differences among the treatment speeds.

4. Discussion

From the micrographs (Figure 3) it is clear that the sanded WPC surface has both wood and

polypropylene components exposed. Both components will interact with the adhesive in different

Page 12: The effect of four methods of surface activation for

ways, relating to their surface energy, level of roughness and chemical functionality of the surface.

The surface energy of polypropylene is typically reported as 30.1 mN m-1 and for wood is 40 to 60

mN m-1, resulting in values of around 31 mN m-1 being recorded for WPCs with PP matrices [26, 27].

Reported values for the surface energy of epoxy resins vary with resin chemistry, but range from

39.1 to 51.6 mN m-1 [28, 29], all of which are higher than the surface free energy of the substrate

material, and indicate that poor wetting will occur. In the control samples of this study, which

received sanding only, it is believed that this exposed the wood particles, and provided surface

roughness for mechanical keying of the adhesive. Previous work [15] showed that there was a

significant increase in adhesion after sanding compared with sample surfaces direct from the

polymer moulding process. Sanding is common practice in wood adhesion, so was adopted

throughout this study, prior to additional treatments.

The adhesion shear strength tests reported here have shown that hydrogen peroxide, hot air and

flame treatment all show an improvement in adhesion strength when used as surface pre-

treatments for WPCs. Only the halogen lamp treatment failed to have a beneficial effect under any

of the parameters studied. For the four treatments evaluated, further work to observe changes in

surface chemistry and surface texture development has also been undertaken but will be reported in

paper 2.

Hydrogen peroxide solutions proved an effective treatment for WPC surface activation in order to

improve its adhesion ability at specific pH values, particularly at pH 6 and 7.5 and 8 but less

significantly at other values tested. This method has been previously reported for bamboo [14], but

not in WPC material. The mechanism is believed to relate to free radical formation on the surface,

which is likely to increase surface energy. WPC materials typically have low surface energies, due to

the matrix polymers used. At pH 7.5 hydrogen peroxide gave an increase in shear strength of 37%

but at this value high variation was encountered (SD=97.53). Curiously there was some activation

either side of neutral pH values but not at neutral (pH 7), and towards the extremes of the pH values

tested the values also decreased. At the optimal value the adhesion was sufficiently strong that

shear failure occurred within the material rather than at the adhesive bond line. Further study of the

different chemical mechanisms acting in the mild acidic and mild alkaline treatment solutions have

been undertaken by FTIR spectroscopy and contact angle analysis, and appear to show significant

differences. The effect of the treatment solution on the wood flour component and on the

polypropylene component within the WPC surface, and resulting effects on the adhesion strength,

will be reported in greater depth in a second paper.

Hot air treatment is also a quick and easy pretreatment to improve WPC adhesion and it is much

faster and easier than hydrogen peroxide treatment because it does not require any chemical

preparation and much less time is needed (few seconds) to obtain similar results. The 115 mm s-1

and 2X75 mm s-1 treatment velocities provided the best surface modification, giving an increase in

bond strength of 38% and 44% respectively, resulting in 50% of the samples showing failure in the

material rather than at the bond line. Low velocities resulted in low bond strengths and little within

material failure which highlights the importance of amount of treatment. The improvement seen in

this study contrasts with the results of Oporto and co-workers [10], who showed a 6% strength loss

in their study which also used epoxy resin. They used a pass speed of 25 mm s-1, but a different heat

gun and the heat was applied from a greater distance (5 cm) from the surface. In the current study,

the use of pre-sanded samples for heat treatment, and the shorter distance from the nozzle of the

heat gun gave a significant increase in bond strength (30%).

Another important factor about the heat treatment is the case of the treatment repetition. It seems

that two passes of the gun with the speed of 75 mm s-1 was a more effective procedure than the

Page 13: The effect of four methods of surface activation for

single pass at any speed. It could be expected that the treatment exposure would be the key factor

for the treatment effectiveness but effectively a 2X75 mm s-1 treatment is equivalent to a speed of

37.5 mm s-1 in terms of overall treatment time. However the slower treatment pass speed resulted

in much lower shear strength than both the 75 mm s-1 and 2X75 mm s-1 samples. It is likely that the

exposure time of the 37.5 mm s-1 causes higher temperature on the surface, which results in lower

adhesion strength than the 2X75 mm s-1. Therefore the repetition might ensure that a more optimal

temperature is achieved for a short duration twice, which is most probably more important for

priming the WPC surface in order to improve the adhesion strength. Initially it was thought that slow

velocities would result in greater surface activation, but the opposite, in terms of bond strength, was

observed. Adhesion mechanisms are a complex system which involves mechanical, chemical and

energetic factors, which interact to affect the adhesion strength. In WPC materials these interactions

are further complicated by the action of heat on two different substrates, with complex results. It is

likely that at faster speeds the beneficial effect of the flame ionisation of the PP surface contributes

to increased lap shear strength, with minimal change to the wood flour component. These factors

have been further investigated using contact angle analysis to determine surface energy, and will be

presented in another paper.

Although the flame treatment gave high mean bond strength values, particularly at velocities slower

than 125 mm s-1, the results were inconsistent, showing high standard deviation at many of the

treatment velocities. At the optimal velocity of 175 mm s-1 it gave a 41% improvement over the

controls, similar to, but slightly lower than, that of the optimal hot air treatment flame (44%

improvement). In terms of variation at these optimal values the flame treatment fared worse, i.e.

flame 782 N at 175 mm s-1 (SD 76.14); hot air 798 N at 2X75 mm s-1 (SD 47.45) and thus is less stable.

The higher variation could be explained by the effect of the flame on the wood flour component of

the WPC. Despite this, the flame treatment is also an effective and quick method to improve the

adhesion strength of the WPC. It does however also require accuracy in selecting the treatment

speed, as incorrect speeds may result to adhesion strength decrease. In industrial flame treaters the

control of feed speed can be well maintained, with Strobel et al [24] reporting typical values of 100

to 300 m min-1 for their experimental studies. In this study the feed speed was slower (7.5 to 15 m

min-1), which may have contributed to higher levels of oxidation and greater variability in properties.

In a workshop preparing small joint areas where the speed is controlled manually there may be a

further increase in the levels of variability seen. In addition, the flame treatment has a medium level

of risk, as it involves applying a flame on flammable materials and there is a greater risk of volatile

emissions. Although the decomposition products of polypropylene itself are relatively harmless; care

should therefore be taken if transferring the technique to other polymers.

Overall the heat treatments applied by hot air gun and flame showed that they were both effective

treatments for improving the adhesion ability of the WPC and also too slow a treatment, i.e.

excessive heating, led to lowered bond strength. Concerning the treatment method efficiency,

Oporto’s study [10] agrees in the case of flame treatment but disagrees with the heat air gun

treatment. It is likely that parameters such as treatment pass speed, proximity of the flame or hot air

source to the substrate surface, and the width of the area receiving flame or hot air treatment, vary

from machine to machine and have significant influence on the level of ionisation which occurs in

the polypropylene component of the WPC material. The same parameters may also influence the

level of thermally induced change in the wood flour component, albeit small in many cases, and

conflict between the beneficial and adverse effects seen in the two components may explain the

suboptimal results observed in some treatment speeds. This area is worthy of greater investigation

and discussion to seek an optimal treatment.

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The halogen heating lamps treatment does not appear to have any advantageous effect on the WPC

adhesion ability. It produces a modified surface that has a reduced adhesion strength, with values

lower than the untreated WPC. This treatment is possibly useful to help us understand the factors

that negatively affect the adhesion strength of the WPC.

5. Conclusions

This study has demonstrated three effective surface pretreatment methods for WPCs: hydrogen

peroxide solutions, hot air and flame. A further treatment using halogen heat lamp failed to show an

improvement in adhesion at any of the speeds studied (10 to 50 mm s-1).

The hydrogen peroxide solutions which showed greatest benefit were pH 6, 7.5, 8 and 8.5. Hydrogen

peroxide at these close to neutral pH values is easily applied and controlled, and offers a simple

system for use in the workshop. A timer and a pH meter is all the equipment required, and the

amount of NaOH which is added into the H2O2 solution for controlling the pH is in very small

quantities that are considered safe [23].

The use of heat for surface activation provided by a hot air gun or from a flame, also improved

adhesive bonding. The majority of conditions studied used single passes of the heat gun or flame

torch. Optimal treatment speeds for the two systems were different – with 115 mm s-1 heat gun and

175 mm s-1 for the flame torch. In the heat gun an additional experiment using two passes at a

slower speed of 75 mm s-1 also showed beneficial results of a similar level.

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